Highlights

• Methane reforming with O₂-containing CO₂ can directly use CO₂ captured from air as raw material.
• Ni-based catalysts optimized by CeO₂-ZrO₂ has smaller Ni particle size and higher Ni dispersion.
• The interaction among Ni, CeO₂ and ZrO₂ results in high reforming activity.
• The optimized Ni-based catalyst owns dual active for methane and CO₂ conversion.

Abstract

Reduction of CO₂ in presence of oxidative impurity (e.g., O₂) is more promising than utilization of pure CO₂ due to skyrocketing cost for purification of captured CO₂ from air or industrial exhaust gas. In this work, Ni-based catalysts are modified by CeO₂ and ZrO₂ to suppress negative effect of O₂ on reforming of CO₂ with methane, which show high CH₄ conversion (97 %) and CO₂ conversion (95 %) at 750 °C and can maintain high CO₂ conversion even with high O₂ content. The physicochemical characterizations on fresh and spent catalysts show that the interaction among Ni, CeO₂ and ZrO₂ results in well dispersion of smaller Ni particles, even after long-term testing. In situ DRIFTS results show that Ni/CeO₂-ZrO₂-SiO₂ catalyst shows advantage to activate CH₄ to generate active CH₃*, promoting the formation of CO, and the CeO₂-ZrO₂ solid solution improves the CO₂ adsorption, thereby reducing the competitive effect of CO₂ and O₂.

The full (paywalled) article appeared on the Applied Catalysis B: Environmental website at https://www.sciencedirect.com/science/article/abs/pii/S0926337321001594